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Activation of metallocene hydride intermediates by methylaluminoxane in alkene dimerization and oligomerization

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Abstract

In order to elucidate the dependence of the structure and reactivity of the bimetallic hydride intermediates formed in the systems metallocene—organoaluminum compound—activator on the nature of the transition metal atom and ligand environment, we used NMR spectroscopy to study reactions of a series of L2MCl2 complexes (M = Hf, Zr; L2 = Cp2, (CpMe)2, ansa-(Me2C)2Cp2, ansa-Me2CInd2) with HAlBui2 and MMAO-12 activator. As a result, M, Al-bimetallic intermediates containing [L2MH3] and [(L2M)2H3] type moieties were detected for both hafnium and zirconium complexes with cyclopentadienyl ligands. The [L2ZrH3] type structure predominates in the system based on the ansa-bis-indenyl zirconium complex. The detected complexes provide associates with MMAO-12 [L2MH3]·MAO and [(L2M)2H3]·MAO. The MAO-associated intermediates of the [(L2M)2H3] type are precursors of the catalytically active sites for alkene dimerization. In the system based on ansa-bis-indenyl zirconium complex, the intermediate of the [L2MH3] type affords a set of hydride structures, presumably cationic, which lead to alkene oligomerization.

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Scheme 1
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Acknowledgements

The structural studies of compounds were carried out at the Center for Collective Use “Agidel” at the Institute of Petrochemistry and Catalysis, Russian Academy of Sciences.

Funding

This research was funded by the Russian Science Foundation, grant number 22-23-00818.

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Authors and Affiliations

  1. Institute of Petrochemistry and Catalysis, Ufa Federal Research Center, Russian Academy of Sciences, Prosp. Oktyabrya, 141, 450075, Ufa, Russian Federation

    Lyudmila V. Parfenova, Pavel V. Kovyazin, Almira Kh. Bikmeeva & Eldar R. Palatov

  2. Department of Chemistry, Lomonosov Moscow State University, 1-3 Leninskiye Gory, 119991, Moscow, Russian Federation

    Pavel V. Ivchenko & Ilya E. Nifant’ev

  3. A.V. Topchiev Institute of Petrochemical Synthesis, Russian Academy of Sciences, Leninsky Prosp. 29, 119991, Moscow, Russian Federation

    Pavel V. Ivchenko & Ilya E. Nifant’ev

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  1. Lyudmila V. Parfenova
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  2. Pavel V. Kovyazin
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  3. Almira Kh. Bikmeeva
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Contributions

All authors have read and agreed to the published version of the manuscript. LVP—conceptualization. PVK—methodology. LVP, PVK and AKB—validation. PVK—formal analysis. PVK, AKB and ERP—investigation. LVP, PVK, PVI and IEN—data curation. PVK—writing—original draft preparation. LVP—writing—review and editing, visualization, supervision, project administration, funding acquisition.

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Parfenova, L.V., Kovyazin, P.V., Bikmeeva, A.K. et al. Activation of metallocene hydride intermediates by methylaluminoxane in alkene dimerization and oligomerization. Reac Kinet Mech Cat 137, 269–286 (2024). https://doi.org/10.1007/s11144-023-02540-7

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